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APPLIED SURFACE SCIENCE · 2022 · IF 7.392

Engineering oxygen vacancies in Co3O4 to boost p-d hybridization for hydrogeneration of nitrogen and oxygen

Xianwei Li,Shuangxiu Ma,Fang Luo,Zehui Yang

Electrochemical hydrogenerations of nitrogen and oxygen molecules are of significance for nitrogen reduction and oxygen reduction reactions. Strengthening the binding between active sites and gaseous molecules is beneficial for enhancing the catalytic performance, especially in NRR catalysis. In this work, we have engineered the oxygen vacancies in Co 3 O 4 nanoparticles to boost the catalytic activity towards NRR and ORR. Ascribing to the p-d hybridization between Co and N atoms, N 2 electrochemical adsorption is promoted and the related energy barrier of N 2 protonation is significantly decreased by 50%; as a consequence, Faradaic efficiency is 11.2% at −0.4 V vs. RHE, 3-fold higher than Co 3 O 4 /CNT; moreover, due to the oxygen vacancies in Co 3 O 4-x /CNT leading to a higher oxophilicity, Co 3 O 4-x /CNT showed a better selectivity in ORR catalysis and kinetic current density at 0.85 V vs. RHE is boosted by 2.4 times. Consequently, Co 3 O 4-x /CNT exhibits a better rechargeable zinc air battery performance than Pt/C-IrO 2 by a factor of 2.2.

研究领域: 材料科学 · 电化学 · 催化科学
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CHEMICAL ENGINEERING JOURNAL · 2016 · IF 5.31

Green preparation and selective permeation of d-Tryptophan imprinted composite membrane for racemic tryptophan

Zhiyong Zhou,Lichao He,Yu Mao,Wenshuai Chai,Zhongqi Ren

Enantioseparation of racemic tryptophan is very important for pharmaceutical production. Conventional separation methods are high costly, energy intensive and environmentally unfriendly. Permeation separation based on membrane separation technique is a promising technology with advantages of energy efficient, clean and no additives. However, lots of organic compounds are commonly used for the traditional preparation of various membranes for enantioseparation of racemic tryptophan. Thus, we developed a totally green and clean preparation method using nature polymer sodium alginate as functional polymer, water as solvent and CaCl 2 as crosslinking agent. Besides, polyvinylidene fluoride membrane was selected as supported membrane. Molecularly imprinted technology with d -Tryptophan as template molecule was introduced to enlarge mass transfer flux. Various methods were used in characterization of molecularly imprinted composite membrane (MICM) and non-imprinted composite membrane (NICM). Effects of preparing conditions, permeation conditions and concentration polarization on permeation performance of MICM by pressure-driven were investigated. High enantiomeric excess ( ee %   >   98%) of the permeation solution could be obtained under mild conditions. Reducing the presence of concentration polarization was beneficial to maintaining high ee % (>98%). Moreover, the thermo and chemical stability of MICM were studied too. Comparison with previous studies indicated that the proposed totally green and clean method was not only low costly and environment friendly but also beneficial to significantly increasing ee .

研究领域: 生物化学 · 制药工程 · 材料科学
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BIOORGANIC CHEMISTRY · 2020 · IF 4.831

New insight into enzymatic hydrolysis of peptides with site-specific amino acid d-isomerization

Liang Yan,Yongqi Ke,Yuhe Kan,Dao Lin,Jingkui Yang,Yujian He,Li Wu

The isomerization of l -amino acids in peptides and proteins into d -configuration under physiological conditions would affect the physiological dysfunction and caused protein conformational diseases. The presence of d -amino acids might change the higher-order structure of proteins and triggered abnormal aggregation. In order to better understand this phenomenon and promote degradation, we systematically studied the enzymatic hydrolysis of a series of peptides obtained by replacing l -amino acids in different positions of template peptide KYNETWRSED with d -amino acids under the action of Protease K. The results showed that, compared with normal peptide, isomerization of different amino acids had different effects on the anti-enzymatic hydrolysis of the peptides, especially d -tryptophan at position 6, which significantly inhibited enzymatic hydrolysis. The analysis of the peptide cleavage site revealed that the efficiency of enzymatic hydrolysis mainly depended on the isomerization of the amino acids at a specific site of the peptide cleavage. Further studies showed that the enzymatic hydrolysis of substrates could be facilitated by optimized reaction conditions such as temperature, pH, addition of metal ions, and change of buffer. In this way the accumulation of disease-associated d -amino acid containing polypeptides/proteins could be prevented.

研究领域: 生物化学 · 分子生物学 · 蛋白质化学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2025 · IF 9.7

Polyaniline-ZnTi-LDH heterostructure with d–π coupling for enhanced photocatalysis of pollutant removal

Chaowei Luo,Jie Xiong,Hongyan Zeng,Mengchen Liao

Heterointerface engineering is an effective strategy to design and construct high-performance photocatalysts. Herein, polyaniline (PANI) nanoparticles and ZnTi layered double hydroxide (ZnTi-LDH) nanosheets were integrated to form organic–inorganic heterostructure (PANI/LDH) via d – π electronic coupling using in-situ polymerization for photocatalytic oxidation/reduction towards tetracycline (TC) and Cr(VI). The photocatalytic activity was closely related to feed amount of aniline (Ani) in the polymerization process, which the abundant PANI nanoparticles were evenly distributed on the surface of ZnTi-LDH nanosheets at the proper Ani feed amount, and thus reinforced d –π electronic coupling at the organic–inorganic interfaces more efficiently. Density functional theory calculations further verified the existence of d –π overlap at the PANI/LDH heterointerface. The strong d –π coupling boosted charge separation and transfer to improve photocatalytic efficiency. As a result, the optimal PANI/LDH (0.3) exhibited outstanding photocatalytic activities with 97.8 % Cr(VI) reducing rate and 87.8 % TC removal rate in the single Cr(VI) and TC system, as well as high simultaneous removal rate of Cr(VI) and TC in TC/Cr(VI) coexistence system, respectively. Subsequently, the photocatalytic enhanced mechanisms were put forward to remove Cr(VI) and TC under visible-light. Finally, the aquatic toxicity of the photolytic products was evaluated using Chlorella sp. as an ecological indicator, showing that the PANI/LDH had a notable detoxification efficiency of TC and Cr(VI).

研究领域: 环境科学 · 材料科学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Triazine-based conjugated polymers with regulation of D-A configuration for enhanced photocatalytic activity

Chengwei Lu,Jun Han,Najun Li,Dongyun Chen,Qingfeng Xu,Hua Li,Jianmei Lu

Photocatalysis is a green and environmentally friendly method for degrading dangerous and nonbiodegradable pollutants. In this study, a sequence of metal-free triazine-based electronic donor–acceptor (D-A) conjugated polymers Tr-X (X = Th, BT, BTh) were prepared by D-A configuration regulation between triazine (Tr) and monomers containing N and S, such as thiophene (Th), bithiophene (BTh) and benzothiadiazole (BT) units, for the photocatalytic degradation of bisphenol A (BPA) and benzene contaminants in water under visible light. Among these, Tr-BTh exhibited complete photocatalytic degradation owing to its excellent D-A configuration. Moreover, the N and S atoms, which are rich in triazine and thiophene units, serve as highly dispersed reactive sites. The separation and transfer of photogenerated carriers can be further improved by expanding the light-absorption range of polymers. In addition, the polymers showed good adsorption for BPA and other aromatic organic pollutants through π-π interaction and surface hydrogen bonding, which provides a facile strategy for efficient polymer-based photocatalysts for water purification.

研究领域: 材料科学 · 环境科学
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Journal of Environmental Chemical Engineering · 2023 · IF 7.7

Biofouling mitigation by D-tyrosine in membrane bioreactor: Short-term performance

Xinying Su,Jintao Luo,Yu Wang,Jinghao Dong,Yu Tian

D -amino acids can inhibit the formation of biofilm without affecting bacterial growth, which is a new strategy to control membrane biofouling. This paper investigated the effects of D -tyrosine on the performance of membrane bioreactor (MBR) during short-term operation. The results showed that the critical flux of activated sludge in MBR increased with the existence of D -tyrosine. The removal efficiencies of wastewater were not affected by D -tyrosine. The fouling propensities of soluble microbial products (SMP) in both MBRs were almost the same. Extracellular polymeric substance (EPS) in D -tyrosine group exhibited weaker fouling propensity. Further research indicated that the addition of D -tyrosine did not have a significant impact on SMP. D -tyrosine lead to the reduction of EPS polysaccharides and the great fluctuation of EPS protein. Microbial community analysis demonstrated that the addition of D -tyrosine changed the microbial community structure in MBR, which might be one of the reasons for the change of EPS.

CAS / MDL: 556-02-5
研究领域: 环境工程 · 微生物学
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Bioengineered · 2017 · IF 1.691

Mining of a phospholipase D and its application in enzymatic preparation of phosphatidylserine

Wen-Bin Zhou,Jin-Song Gong,Hai-Juan Hou,Heng Li,Zhen-Ming Lu,Hong-Yu Xu,Zheng-Hong Xu,Jin-Song Shi

Phosphatidylserine (PS) is useful as the additive in industries for memory improvement, mood enhancement and drug delivery. Conventionally, PS was extracted from soybeans, vegetable oils, egg yolk, and biomass; however, their low availability and high extraction cost were limiting factors. Phospholipase D (PLD) is a promising tool for enzymatic synthesis of PS due to its transphosphatidylation activity. In this contribution, a new and uncharacterized PLD was first obtained from GenBank database via genome mining strategy. The open reading frame consisted of 1614 bp and potentially encoded a protein of 538-amino-acid with a theoretical molecular mass of 60 kDa. The gene was successfully cloned and expressed in Escherichia coli. Its enzymatic properties were experimentally characterized. The temperature and pH optima of PLD were determined to be 60°C and 7.5, respectively. Its hydrolytic activity was improved by addition of Ca2+ at 5 mM as compared with the control. The enzyme displayed suitable transphosphatidylation activity and PS could be synthesized with L-serine and soybean lecithin as substrates under the catalysis of PLD. This PLD enzyme might be a potential candidate for industrial applications in PS production. To the best of our knowledge, this is the first report on genome mining of PLDs from GenBank database.

CAS / MDL: 56-45-1
研究领域: 生物化学 · 分子生物学 · 工业酶学
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JOURNAL OF COLLOID AND INTERFACE SCIENCE · 2024 · IF 9.4

Optimizing photocatalytic hydrogen evolution performance by rationally constructing S-scheme heterojunction to modulate the D-band center

Zhiliang Jin,Cheng Yang

The research in the field of photocatalysis has progressed, with the development of heterojunctions being recognized as an effective method to improve carrier separation efficiency in light-induced processes. In this particular study, CuCo 2 S 4 particles were attached to a new cubic CdS surface to create an S-scheme heterojunction, thus successfully addressing this issue. Specifically, owing to the higher conduction band and Fermi level of CuCo 2 S 4 compared to CdS, they serve as the foundation and driving force for the formation of an S-scheme heterojunction. Through in-situ X-ray photoelectron spectroscopy and electron paramagnetic resonance analysis, the direction of charge transfer in the composite photocatalyst under light exposure was determined, confirming the charge transfer mechanism of the S-scheme heterojunction. By effectively constructing the S-scheme heterojunction, the d-band center of the composite photocatalyst was adjusted, reducing the energy needed for electron filling in the anti-bonding energy band, promoting the transfer of photogenerated carriers, and ultimately enhancing the photocatalytic hydrogen production . performance. After optimization, the hydrogen evolution activity of the composite photocatalyst CdS-C/CuCo 2 S 4 -3 reached 5818.9 μmol g −1 h −1 , which is 2.6 times higher than that of cubic CdS (2272.3 μmol g −1 h −1 ) and 327.4 times higher than that of CuCo 2 S 4 (17.8 μmol g −1 h −1 ), showcasing exceptional photocatalytic activity. Electron paramagnetic resonance and in situ X-ray photoelectron spectroscopy have established a theoretical basis for designing and constructing S-scheme heterojunctions, offering a viable method for adjusting the D-band center to enhance the performance of photocatalytic hydrogen evolution.

CAS / MDL: 13963-58-1
研究领域: 材料科学 · 能源化学 · 环境科学
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FUEL · 2025 · IF 7.5

Constructing CoFe alloy and tailoring d-band center in trimetallic ZIF-derived porous carbon for bifunctional oxygen electrocatalysis

Yanan Ma,Dingyu Zhang,Haimeng Wang,Yuxuan Liang,Yuan Zhang,Fengfeng Yan,Liang Sun,Qian Wang,Wei Li

Synthesis of multiple-site single-atom catalyst (SAC) with metal-containing nanoparticles by using zeolite imidazole framework (ZIF) for improving the bifunctional electrocatalytic performance is of great significance, yet it is also a challenge. Trimetallic ZIF-derived porous carbon nanosheets with the CoFe alloy nanoparticles enclosed in nitrogen-doped carbon nanotubes (N-CNTs) are fabricated by utilizing three transition metals as ZIF precursors and sodium chloride as templates via a typical two-step process, including synthesis and pyrolysis. By building CoFe alloy and tailoring d-band center ( E d ) of the Co site, the as-obtained FeCoZn@S-CN ZIF exhibits predominant kinetic activity and durability towards ORR and OER with an extremely low potential gap (Δ E ) value of 0.584    V, exceeding many other efficient counterparts. This study provides an effective approach for designing and synthesizing atomically dispersed multi-metal site catalysts with alloyed nanoparticles to achieve high-efficient bifunctional electrocatalytic performance in the application of the recharged zinc-air battery (ZAB).

研究领域: 材料科学 · 电化学
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APPLIED MICROBIOLOGY AND BIOTECHNOLOGY · 2018 ·Vol. 102 ·期 14 ·6039-6046 · IF 3.34

A highly active pantothenate synthetase from Corynebacterium glutamicum enables the production of d-pantothenic acid with high productivity

Tigu Fitsum,Zhang Junli,Liu Guoxia,Cai Zhen,Li Yin

d -Pantothenic acid (vitamin B 5 ) has wide applications in the feed, food, chemical, and pharmaceutical industries. Its biological production routes which employ pantothenate synthetase (PS) as the key enzyme are attractive since they avoid the tedious and time-consuming optical resolution process. However, little data is available on the activity and kinetics of this enzyme, hampering the rational selection of an efficient enzyme for the biological production of d -pantothenic acid. In this study, six phylogenetically distant PS-encoding genes, from Escherichia coli , Corynebacterium glutamicum , Bacillus subtilis , Bacillus thuringiensis , Bacillus cereus , and Enterobacter cloacae , were expressed in E. coli . The PS from C. glutamicum exhibited a specific activity of 205.1 U/mg and a turnover number of 127.6 s -1 , which to our best knowledge are the highest values ever reported. The addition of substrates ( d -pantoic acid and β-alanine) to the E. coli strain harboring this enzyme during the early log phase of fermentation resulted in the production of 97.1 g/L of d -pantothenic acid within 32 h, corresponding to a conversion yield of 99.1% and a productivity of 3.0 g/L/h. To the best of our knowledge, this is the highest productivity reported to date.

CAS / MDL: 50-99-7
研究领域: 生物化学 · 微生物学 · 工业生物技术
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GREEN CHEMISTRY · 2018 ·Vol. 20 ·期 10 ·2320-2327 · IF 8.586

Enzymatic hydrolysis of chitin pretreated by bacterial fermentation to obtain pure N-acetyl-D-glucosamine

Alei Zhang,Guoguang Wei,Xiaofang Mo,Ning Zhou,Kequan Chen,Pingkai Ouyang

In this study, we propose a novel biological fermentation method to process chitin powder utilizing the bacteria Chitinolyticbacter meiyuanensis SYBC-H1. The chitin obtained from this process is called CBF, and it was further investigated for N-acetyl-D-glucosamine (GlcNAc) enzymatic production. This fermentative treatment caused chitin powder to acquire a visible fleecy structure, and scanning electron microscopy showed that the surface of the CBF was a fiber-like structure with a diameter ranging from 10 nm to 200 nm. Moreover, Fourier transform infrared spectrometry, X-ray diffraction and gel permeation chromatography revealed that the crystallinity and average molecular weight of the chitin clearly decreased in the absence of deacetylation following bacterial fermentation treatment. The optimal conditions for bacterial treatment of chitin were determined at 25 °C, 200 rpm, and an initial pH of 7.5 for 12 h. Additionally, 19.2 g L−1 of GlcNAc could be obtained with a yield of 96% from 20 g L−1 of CBF in a batch enzymatic reaction within 6 h. This new approach provided an environmentally friendly and mild method for reducing the crystallinity of chitin and enhancing GlcNAc conversion without the use of oxidants, acids, or other environment unfriendly reagents.

研究领域: 生物化学 · 微生物学 · 环境科学
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ANALYTICAL LETTERS · 2024 · IF 1.6

A Dual-Mode Optical Sensing Strategy for Rapid Detection of D-Penicillamine in Pharmaceutical Formulations

Jin-Wen Liu,Tingting Chen,Meiqun Cai,Yingfeng Qin,Mei Li

Accurate, rapid, and quantitative detection of D-penicillamine (D-PA) in pharmaceutical formulations is imperative for drug quality and clinical medication guidance. Various colorimetric and fluorescent assays have been constructed for D-PA based on nanomaterials. However, the reliable and rapid detection of D-PA in pharmaceutical formulations remains a challenge because these methods suffer from shortcomings such as time-consuming procedures, poor uniformity, and complicated nanomaterial preparation. In this work, an effective and facile homogeneous dual-mode optical sensing strategy was established based on the strong complexation between D-PA and Cu2+ and catalyzed the oxidation of O-phenylenediamine. This platform displayed a sensitive response to D-PA from 5 to 100 µmol/L, with a detection limits of 0.54 µmol/L (fluorescence) and 0.76 µmol/L (colorimetry). As expected, the method was successfully applied to the determination of D-PA in pharmaceutical formulations with satisfactory results. Overall, this developed strategy provides a facile and rapid dual-mode optical platform for D-PA and has great potential in D-PA-related pharmaceutical quality control.

研究领域: 分析化学 · 药学
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